WO2023279312A1 - Capteur de micro-analyte - Google Patents

Capteur de micro-analyte Download PDF

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Publication number
WO2023279312A1
WO2023279312A1 PCT/CN2021/105112 CN2021105112W WO2023279312A1 WO 2023279312 A1 WO2023279312 A1 WO 2023279312A1 CN 2021105112 W CN2021105112 W CN 2021105112W WO 2023279312 A1 WO2023279312 A1 WO 2023279312A1
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WO
WIPO (PCT)
Prior art keywords
micro
electrode
analyte sensor
layer
analyte
Prior art date
Application number
PCT/CN2021/105112
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English (en)
Inventor
Cuijun YANG
Original Assignee
Medtrum Technologies Inc.
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Medtrum Technologies Inc. filed Critical Medtrum Technologies Inc.
Priority to EP21948810.3A priority Critical patent/EP4366618A1/fr
Priority to PCT/CN2021/105112 priority patent/WO2023279312A1/fr
Publication of WO2023279312A1 publication Critical patent/WO2023279312A1/fr

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    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B5/00—Measuring for diagnostic purposes; Identification of persons
    • A61B5/145—Measuring characteristics of blood in vivo, e.g. gas concentration, pH value; Measuring characteristics of body fluids or tissues, e.g. interstitial fluid, cerebral tissue
    • A61B5/14532—Measuring characteristics of blood in vivo, e.g. gas concentration, pH value; Measuring characteristics of body fluids or tissues, e.g. interstitial fluid, cerebral tissue for measuring glucose, e.g. by tissue impedance measurement
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B5/00—Measuring for diagnostic purposes; Identification of persons
    • A61B5/145—Measuring characteristics of blood in vivo, e.g. gas concentration, pH value; Measuring characteristics of body fluids or tissues, e.g. interstitial fluid, cerebral tissue
    • A61B5/1486—Measuring characteristics of blood in vivo, e.g. gas concentration, pH value; Measuring characteristics of body fluids or tissues, e.g. interstitial fluid, cerebral tissue using enzyme electrodes, e.g. with immobilised oxidase
    • A—HUMAN NECESSITIES
    • A61—MEDICAL OR VETERINARY SCIENCE; HYGIENE
    • A61B—DIAGNOSIS; SURGERY; IDENTIFICATION
    • A61B2562/00—Details of sensors; Constructional details of sensor housings or probes; Accessories for sensors
    • A61B2562/02—Details of sensors specially adapted for in-vivo measurements
    • A61B2562/0209—Special features of electrodes classified in A61B5/24, A61B5/25, A61B5/283, A61B5/291, A61B5/296, A61B5/053

Definitions

  • the invention mainly relates to the field of medical devices, in particular to a micro analyte sensor.
  • the pancreas in a normal human body can automatically monitor the level of glucose in the human blood and automatically secrete the required insulin/glucagon.
  • the pancreas does not function properly and cannot produce the insulin the body needs. Therefore, diabetes is a metabolic disease caused by abnormal pancreatic function, and diabetes is a lifelong disease. At present, there is no cure for diabetes with medical technology. The occurrence and development of diabetes and its complications can only be controlled by stabilizing blood glucose.
  • Diabetics need to have their blood glucose measured before they inject insulin into the body. At present, most of the testing methods can continuously measure blood glucose and send the data to a remote device in real time for the user to view. This method is called Continuous Glucose Monitoring (CGM) .
  • CGM Continuous Glucose Monitoring
  • the method requires the device to be attached to the skin and the probe it carries is inserted into the tissue fluid beneath the skin.
  • the present invention implementation example first published in a micro analyte sensor, including at least one electrode group, electrode group includes at least one working electrode and at least one additional electrodes, the working electrode’s and/or additional electrode’s electrical conduction layer sets at least one surface micro structure,
  • the adhesive force between the electron conduction layer and the substrate and membrane layer can be improved, and the processing cost is lower.
  • the invention discloses a micro analyte sensor, which comprises the substrate, the substrate comprises an internal part and an external part; At least one electrode group located on the surface of the internal part , the electrode group includes at least one working electrode and at least one additional electrode; The external part is provided with a PAD corresponding to each electrode, and the PAD is electrically connected with the working electrode and the additional electrode respectively through a wire; At least one surface of the working electrode and/or the additional electrode is provided with a micro structure.
  • the electron conduction layer of the working electrode and the counter electrode is platinum.
  • the micro structure includes either a micro-groove or a micro-bulge.
  • the micro-groove includes one or more of a micro-through-hole or a micro-blind hole or a micro-notch.
  • the micro-structure has a diameter of 0.001 ⁇ 100um.
  • the density of the micro structure is 1*10 2 ⁇ 1*10 10 /cm 2 .
  • the material of the substrate is selected from one or more combinations of polytetrafluoroethylene, polyethylene, polyvinyl chloride, acrylonitrile-butadiene-styrene copolymer, polymethyl methacrylate, polycarbonate and polyimide.
  • the micro analyte sensor is provided with a working electrode and an additional electrode in the internal part of the substrate, and all the electrodes are electrically connected with the corresponding PAD arranged in the internal part through a wire.
  • At least one surface of the electronic conduction layer of the working electrode and/or the additional electrode is provided with a micro structure to increase the surface area and roughness of the electronic conduction layer, enhance the adhesion force of the electrode and improve the detection reliability of the sensor , so it can increase adhesive force between the electrical conduction layer and substrate, membrance layer, thus it reduces the possibility that the electrode and the membrance layer may shift or fall off during use, improve the reliability of the sensor.
  • the micro analyte sensor disclosed in the invention can be divided into a three-electrode system and a two-electrode system, wherein the three-electrode system consists of a counter electrode, a reference electrode and at least one working electrode, and the two-electrode system consists of a counter electrode and at least one working electrode.
  • the invention can also be divided into two situations: 1) single working electrode: there is only one working electrode; 2) Dual working electrode: there are two working electrodes, one of which is called “working electrode” for electroredox reaction with analyte to generate electrical signal, and the other is usually responsible for detecting the response signal of interference or background solution, called “auxiliary electrode” .
  • the three-electrode system can effectively control the detection potential, prevent potential drift, and improve the reliability of the parameter information of the detection analyte.
  • the two-electrode system has simple structure and lower production cost.
  • the electron conduction layer of each electrode is made of materials with good conductivity and strengthening inert as the electrode material.
  • precious metal materials such as gold, platinum and silver become the better choice.
  • both the working electrode and the counter electrode are platinum.
  • the electrical conduction layer on the surface of the micro structure can be micro grooves, can also be a tiny bumps, when the micro structure is a micro grooves, can be a tiny hole or tiny blind holes or micro indentation, one or more of that micro structures are not limited to its own specific shape, can increase the surface area and roughness, reduce the requirements of processing technology and processing costs.
  • the substrate material of the sensor is selected from one or more combinations of polytetrafluoroethylene (TEFLON) , polyethylene (PE) , polyvinyl chloride (PVC) , acrylonitrile-butadiene-styrene copolymer (ABS) , polymethyl methacrylate (PMMA) , polycarbonate (PC) , polyimide (PI) , etc. All of the above materials have excellent insulating properties, water impermeability and high mechanical strength, which can extend the service life of the sensor.
  • TEFLON polytetrafluoroethylene
  • PE polyethylene
  • PVC polyvinyl chloride
  • ABS acrylonitrile-butadiene-styrene copolymer
  • PMMA polymethyl methacrylate
  • PC polycarbonate
  • PI polyimide
  • the second aspect of the present invention discloses a continuous analyte monitoring device, which comprises a bottom shell for mounting on the skin surface of the host.
  • the sensor unit comprises a base and at least one micro analyte sensor as described above.
  • the micro analyte sensor is fixed on the base, and the sensor unit is installed on the bottom shell through the base to detect the analyte parameter information in the host body.
  • the transmitter is electrically connected with the sensor unit for sending the parameter information of the analyte to the outside world.
  • a battery which is used to provide electrical energy.
  • a receiver which is used to receive analyte parameter information and indicate to the user.
  • Fig. 1 is a structural schematic diagram of a sensor according to an embodiment of the invention.
  • Fig. 2 is a side view of the sensor in the embodiment of Fig. 1;
  • Fig. 3 shows a sectional view of the electrode
  • Fig. 4 is a schematic diagram of the micro structure of the surface of the electron conduction layer according to an embodiment of the invention.
  • Fig. 5 is the V-V 'profile of Fig. 4;
  • the adhesion between the electrode electron conduction layer and the substrate and the membrance layer of the analyte sensor with the existing technology is weak, and the electrode and the membrance layer are easy to shift or fall off during the use, which affects the reliability of the sensor.
  • the invention provides a micro analyte sensor, which is arranged on the surface of the internal part on the substrate with at least one electrode group, the electrode group comprises at least one working electrode and at least one additional electrode, and all the electrodes are electrically connected with the corresponding PAD arranged on the internal part through a wire.
  • the working electrode’s and the additional electrode’s electrical conduction layer surface is set with micro structure, so as to increase the surface area of electrical conduction layer at the same time, also increased the roughness of the surface, therefore, the adhesive force between the electron conduction layer, the substrate and the membrance layer can be increased, which reduces the possibility of the electrode and the membrance layer shifting or falling off in the process of use, and improves the reliability of the sensor .
  • one or more method steps referred to in the present invention do not exclude the possibility that other method steps may exist before and after the combined steps or that other method steps may be inserted between such explicitly mentioned steps, unless otherwise stated.
  • the combination connection between one or more devices/devices referred to in the invention does not preclude the existence of other devices/devices before and after the said combination devices or the insertion of other devices between the two specifically mentioned devices, unless otherwise stated.
  • Fig. 1 is the structural schematic diagram of the sensor in the embodiment of the invention
  • Fig. 2 is a side view of the sensor in the embodiment of Fig. 1.
  • Sensor 11 includes the base 111, which is divided into an external part X and an internal part Y as shown in Fig. 1 with dotted lines as the dividing line.
  • the internal part Y electrode including at least one of the working electrode 1131 and at least one additional electrodes, obviously, in this example, additional electrodes include counter electrode 1231 and reference electrode 1331, which constitute three-electrodes system, the counter electrode 1231 is opposite to the working electrode 1131, it forms a closed loop with the working electrode 1131, so that the current on the electrode can conduct normally.
  • the reference electrode 1331 is used to provide the reference potential of the working electrode 1131, so that the detection potential can be effectively controlled.
  • additional electrodes may also include counter electrode 1231 only, so as to form a two-electrode system, compared to the three-electrode system, the effective area of working electrode 1131 and counter electrode 1231 can be increased on the limited area of internal part Y, so as to prolong the service life of the electrode, and because one electrode is removed, the process is simpler.
  • working electrode 1131 does not have the detection potential of the reference electrode as a reference, so the reliability of the detection information of the analyte will be reduced.
  • the working electrode 1131 has at least two, one of which generates an electrical signal by electroredox reaction with the analyte to be detected, and the other is used to detect the response signal of interference or background solution in the body fluid of the host, which called auxiliary electrode.
  • the external part X is provided with a PAD , which corresponds to the electrode one-to-one and is electrically connected through a wire, that is, the first PAD1111 corresponding to the working electrode 1131 is electrically connected through wire 1121, the second PAD1211 corresponding to the counter electrode 1231 is electrically connected through wire 1221, and the third PAD1311 corresponding to the reference electrode 1331 is electrically connected through wire 1321.
  • the different pads, wires, and electrodes are insulated from each other to prevent interference with electrical signals.
  • the fifth PAD 1212 corresponding to the counter electrode 1232 is electrically connected through wire 1222.
  • the sixth Pad 1312 corresponding to the reference electrode 1332 electrically connected through wire 1322.
  • the pads, wires, and electrodes on both surfaces may be symmetrically or asymmetrically arranged.
  • the corresponding PAD, wire and electrode are laid on the same surface or can be laid on different surfaces.
  • the corresponding PAD, wire and electrode are laid on the same surface to facilitate the wiring of the wire.
  • the position of the working electrode 1131 on surface A can be changed with that of the counter electrode 1231 on surface A, or the position of the counter electrode 1231 on surface A can be changed with that of the reference electrode 1332 on plane B.
  • the service life of the sensor can be further extended by increasing the number of electrode groups by increasing the sensor area or decreasing the electrode area, although the planar structure sensor only has relative surface A and surface B.
  • too large sensor area may increase the host's rejection reaction and cause the host's discomfort. Too small electrode area will reduce the sensitivity of the electrode and reduce the reliability of the detection parameters.
  • An excessive number of electrode groups will also increase the complexity of the processing process, for example, the wiring of the wire will become very dense. Therefore, it is preferred that the number of electrode groups be two.
  • each electrode group may also be distributed on the same surface of the sensor, such as surface A or surface B, without limitation herein.
  • the substrate 111 is a material with excellent insulating properties, mainly from inorganic non-metallic ceramics, silica glass and organic polymers, etc.
  • the substrate material is also required to have high water permeability and mechanical strength.
  • the substrate materials are selected from one or more combinations of polytetrafluoroethylene (Teflon) , polyethylene (PE) , polyvinyl chloride (PVC) , acrylonitrile-butadiene-styrene copolymer (ABS) , polymethyl methacrylate (PMMA) , polycarbonate (PC) , polyimide (PI) , etc.
  • the electron conduction layer a is made of materials with good electrical conductivity and fortification inertia.
  • the working electrode and the counter electrode are selected from graphite electrode, glass carbon electrode, noble metal and other materials
  • the reference electrode is selected from one of Ag/AgCl or calomel.
  • noble metal electrodes such as gold electrode, platinum electrode and silver electrode, become a better choice.
  • the working electrode and counter electrode are both platinum electrode for further optimization.
  • the micro structure is arranged in the electron conduction layer a.
  • the anti-interference layer b is located between the enzyme layer and the electron conduction layer.
  • Interferers are molecules or substances that undergo electrochemical reduction or oxidation on the electrode surface, either directly or indirectly through an electron transfer agent, resulting in an erroneous signal that interferes with analyte detection. For example, for the determination of glucose as an analyte, common interferences in the body are urea, ascorbic acid, acetaminophen, and so on.
  • the anti-interference layer b prevents one or more interference agents from penetrating the electrolyte surrounding the electrode.
  • the anti-interference layer b allows the analyte to be measured at the electrode (e.g., hydrogen peroxide) to pass through, while at the same time preventing the passage of other substances (e.g., potentially interfering substances) .
  • the anti-interference layer b could be a very thin membrance designed to limit the diffusion of substances with molecular weights greater than 34Da.
  • the anti-interference layer b can be an organic polymer, which can be prepared from organosilane and a hydrophilic copolymer.
  • Hydrophilic copolymers preferably, polyethylene glycol (PEG) , poly (2-hydroxyethyl methacrylate) and poly (lysine) .
  • the thickness of the anti-interference layer b may range from 0.1 um or less to 10 um or more. The preferred thickness range is 0.5 um to 5 um.
  • the upper limit of the sensor's linear response to glucose is only about 40mg/dL. However, in a clinical setting, the upper limit of the linear response of blood glucose levels needs to be about 500mg/dL.
  • Adjustment layer d acts primarily as a semi-permeable membrane to regulate the amount of oxygen and glucose transmitted to the enzyme layer and, more specifically, to make oxygen excess a non-limiting factor.
  • the upper limit of the linear response of the sensor to glucose with the adjustment layer can be reached to a higher level than that without the adjustment layer.
  • the ratio of oxygen-glucose transmittance in adjustment layer d can be reached to 200: 1, thus ensuring that sufficient oxygen is available for the enzymatic reaction at any glucose and oxygen concentration that may be present subcutaneally.
  • the adjustment layer d may be an organic polymer, which may be prepared from organosilane and a hydrophilic copolymer. Hydrophilic copolymer, preferably, copolymerization or graft of polyethylene glycol (PEG) . Other hydrophilic copolymers that may be used include, but are not limited to, other diols such as propylene glycol, esters, amides, carbonates, and polypropylene glycol. The use of organosilicone polymers can obviously improve the oxygen transmission, and effectively control the glucose transmission.
  • the adjustment layer d may be in the thickness range of 1 um or less to 50 um or greater, with a preferred thickness range of 1 um to 10 um.
  • the biocompatibility layer e is located at the outermost part of the electrode, which is designed to eliminate the body's rejection of foreign bodies and reduce the formation of a shielding cell layer around the implanted electrode.
  • the biocompatibility layer e can be prepared from organosilanes and a hydrophilic copolymer.
  • Hydrophilic copolymer preferably, copolymerization or graft of polyethylene glycol (PEG) .
  • PEG polyethylene glycol
  • Other hydrophilic copolymers that may be used include, but are not limited to, other diols such as propylene glycol, esters, amides, carbonates, and polypropylene glycol.
  • the thickness of the biocompatibility layer e may range from 1 micron or less to 100 microns or more.
  • a preferred thickness range is 10 um to 30 um.
  • Fig. 4 is a schematic diagram of the electrode surface micro-structure of an embodiment of the invention
  • Fig. 5 is the V-V 'profile of Fig. 4.
  • the electronic conduction layer a of the electrode is divided into surface A and surface B.
  • One side is attached to the base 11 of the sensor, and the other side is attached to the membrane layer (b ⁇ c ⁇ d ⁇ e) .
  • membrane layer (b ⁇ c ⁇ d ⁇ e) There are micro structures on both sides, which can increase the roughness of the surface on the other hand, in order to enhance the electrical conduction layer a and a base 11, membrane layer (b ⁇ c ⁇ d ⁇ e) , the adhesion force, prevent when use, the electrode on the basal or membrane layer between shift or fall off, at the same time also can enhance the electrode with polymer, such as the adhesion strength of the glucose in the body, improve the reliability and stability of the sensors.
  • micro bulges such as micro bulges 11311a, 11311b, 11311c, etc.
  • the micro bulges have no specific shape restrictions, and can be tri-prismatic, spherical, rectangular or irregular, with a diameter of 0.001 ⁇ 100um, which is preferred. The diameter is 10 ⁇ 50um.
  • micro-grooves are formed by concave micro-structures inside the surface of electron conduction layer a, such as micro-grooves 11311d, 11311e and 11311f.
  • the micro-bulges can be tri-prismatic, spherical, rectangular or irregular. Shapes such as the notch of a strip (not shown) .
  • the diameter of the micro grooves is 0.001 ⁇ 100um, and the height of the micro bulge or the depth of the micro grooves is 0. 001 ⁇ 50um.
  • the diameter is 10 ⁇ 50um, the height of the micro bulge or the depth of the micro groove is 10 ⁇ 30um.
  • the micro bulges or micro grooves on either side of the electron conduction layer a, they can be evenly arranged according to the interval of equal height or equal width, or they can be randomly arranged, and no restriction is made herein.
  • its density needs to be limited to a certain range, such as 1*10 2 ⁇ 1*10 10 /cm 2 , too large or too small of the micro structure density can not achieve the desired effect of increasing adhesion force.
  • micro bulges or micro grooves may be obtained by means of chemical etching.
  • chemical etching For example, through the process of cleaning -chemical solution (HCl/C 2 H 2 O 2 /NH 4 Cl/FeCl 3 ) corrosion -cleaning -brightening treatment -cleaning -drying treatment, can be obtained about 1 ⁇ 50 um in diameter, density 5*10 2 ⁇ 3*10 3 /cm 2 , thickness of 1 ⁇ 10 um micro convex or micro groove.
  • the laser etching process can also be used to control the laser stroke and energy to obtain the micro bump or micro groove as the above parameters.
  • the process of producing micro-grooves or micro-bulges is simpler and less costly than that of producing platinum black.
  • the electron conduction layer a is also provided with a carbon nanotube modified layer (not shown in the figure) .
  • the carbon nanotubes are modified to the surface of the electron conduction layer a on the surface of the formed electron conduction layer a by means of physical adsorption, embedding or covalent bonding to improve the electron transfer speed.
  • the modified carbon nanotube layer can be fixed on the surface of the electron conduction layer a by Nafion solution dispersion method, covalent fixation method, etc.
  • the invention discloses a micro analyte sensor, which is provided with at least one electrode group arranged on the surface of the internal part on the substrate, and the electrode group comprises at least one working electrode and at least one additional electrode. All the electrodes are electrically connected with the corresponding PAD arranged in the internal part through a wire.
  • Working electrode and the additional electrical conduction layer surface of the electrode is set with micro structure, increase the surface area of electrical conduction layer at the same time, also increased the roughness of the surface, therefore, the adhesion force between the electron conduction layer and the substrate and membrane layer can be increased, it reduces the possibility of electrode and membrance layer shifting or falling off in the process of use and improves the reliability of the sensor .

Abstract

Capteur de micro-analyte (11) comprenant une base (111) qui comprend une partie interne (Y) et une partie interne (X). Au moins un groupe d'électrodes est situé sur la surface de la partie interne (Y) et chaque groupe d'électrodes comprend au moins une électrode de travail (1131) et au moins une électrode supplémentaire (1231, 1331). La partie interne (X) est pourvue d'un PAD (1111, 1211, 1311) correspondant à chaque électrode et le PAD (1111, 1211, 1311) est électriquement connecté à l'électrode de travail (1131) et à l'électrode supplémentaire (1231, 1331) respectivement à travers un fil (1121, 1221, 1321). Au moins une surface de la couche de conduction électronique de l'électrode de travail (1131) et/ou de l'électrode supplémentaire (1231, 1331) est pourvue d'une micro-structure (11311) pour augmenter la surface et la rugosité de la couche de conduction électronique (a), améliorer la force d'adhérence de l'électrode et améliorer la fiabilité de détection du capteur.
PCT/CN2021/105112 2021-07-08 2021-07-08 Capteur de micro-analyte WO2023279312A1 (fr)

Priority Applications (2)

Application Number Priority Date Filing Date Title
EP21948810.3A EP4366618A1 (fr) 2021-07-08 2021-07-08 Capteur de micro-analyte
PCT/CN2021/105112 WO2023279312A1 (fr) 2021-07-08 2021-07-08 Capteur de micro-analyte

Applications Claiming Priority (1)

Application Number Priority Date Filing Date Title
PCT/CN2021/105112 WO2023279312A1 (fr) 2021-07-08 2021-07-08 Capteur de micro-analyte

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WO2023279312A1 true WO2023279312A1 (fr) 2023-01-12

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Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104761697A (zh) * 2014-01-02 2015-07-08 上海移宇科技有限公司 一种生物传感器的膜层及制备方法
CN104825171A (zh) * 2009-02-26 2015-08-12 雅培糖尿病护理公司 改进的分析物传感器及其制造和使用方法
US20190008425A1 (en) * 2017-03-17 2019-01-10 Medtronic Minimed, Inc. Metal pillar device structures and methods for making and using them in electrochemical and/or electrocatalytic applications
CN110678122A (zh) * 2017-05-11 2020-01-10 美敦力泌力美公司 分析物传感器和用于制造分析物传感器的方法
CN111096754A (zh) * 2019-12-31 2020-05-05 上海硕创生物医药科技有限公司 一种生物传感器
CN111742215A (zh) * 2018-04-09 2020-10-02 加州理工学院 金属-酶夹层
US20210145352A1 (en) * 2017-06-02 2021-05-20 Northwestern University Epidermal sensing systems for optical readout, visualization and analysis of biofluids

Patent Citations (7)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
CN104825171A (zh) * 2009-02-26 2015-08-12 雅培糖尿病护理公司 改进的分析物传感器及其制造和使用方法
CN104761697A (zh) * 2014-01-02 2015-07-08 上海移宇科技有限公司 一种生物传感器的膜层及制备方法
US20190008425A1 (en) * 2017-03-17 2019-01-10 Medtronic Minimed, Inc. Metal pillar device structures and methods for making and using them in electrochemical and/or electrocatalytic applications
CN110678122A (zh) * 2017-05-11 2020-01-10 美敦力泌力美公司 分析物传感器和用于制造分析物传感器的方法
US20210145352A1 (en) * 2017-06-02 2021-05-20 Northwestern University Epidermal sensing systems for optical readout, visualization and analysis of biofluids
CN111742215A (zh) * 2018-04-09 2020-10-02 加州理工学院 金属-酶夹层
CN111096754A (zh) * 2019-12-31 2020-05-05 上海硕创生物医药科技有限公司 一种生物传感器

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